文献类型：期刊文献

英文题名：AuCu Nanodendrite for Enhancing Electrocatalytic Nitrate Reduction Applications via Two-stage Microfluidic Fabrication Strategy

作者：Liu, Hengyuan[1];Jia, Yongqi[2];Huang, Xintong[2];Liu, Yingzhe[3];Yang, Qiang[1];Chen, Zhuo[2];Xu, Jianhong[2]

机构：[1]East China Univ Sci & Technol, Sch Mech & Power Engn, Shanghai 200237, Peoples R China;[2]Tsinghua Univ, Dept Chem Engn, State Key Lab Chem Engn, Beijing 100084, Peoples R China;[3]Xiamen Univ Technol, Sch Mech & Automot Engn, Xiamen 361024, Peoples R China

年份：2025

卷号：15

期号：2

起止页码：1230

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20250217659602);WOS:【SCI-EXPANDED(收录号:WOS:001391427600001)】；

基金：This work was supported by the National Natural Science Foundation of China (22025801, 22208190, 22308186) and a Sinopecfund (122096).

语种：英文

外文关键词：AuCu alloy; dendritic structure; controllablefabrication; microfluidic strategy; electrocatalyticnitrate reduction reaction

摘要：The electrocatalytic nitrate reduction reaction (NitrRR) has attracted great attention in clean ammonia production, but it has unsatisfactory selectivity and sluggish dynamics, owing to the complex eight-electron transfer process. While dendritic AuCu alloy is anticipated to offer competitive performance, significant challenges remain in terms of insufficient structural regulation and an unelucidated reaction enhancement mechanism because of the complexity involved in its preparation. To address these issues, we have developed a two-stage microfluidic platform that facilitates the stable fabrication and controllable regulation of AuCu nano dendrites (NDs). Notably, the Cu content in the resultant AuCu NDs reaches an impressive 35.34 At%, surpassing traditional liquid-phase reduction limitations. Furthermore, the dendrite structure has been thoroughly validated, revealing a clear structure-activity relationship. By employing precise manipulation, we have determined the optimal composition of AuCu NDs, achieving a remarkable ammonia yield of 21.93 mg h-1 cm-2 and a faradic efficiency of 93.30%. Additionally, DFT calculations further elucidate the performance enhancement mechanism, showing that Au3Cu1 sites in the AuCu NDs significantly reduce the energy barrier (0.28 eV) of the rate-determining step (RDS: *NO -> *HNO), while excessive Cu deposition has an adverse effect. Our work contributes innovative guidance for the design and controllable fabrication of high-performance electrocatalysts.